Titanium
nitride is a refractory material with excellent thermal
and mechanical stabilities as well as optical and plasmonic properties
in the visible and near-infrared (NIR) regions. Alloying different
concentrations of aluminum element in TiN can not only change the
dielectric properties from metallic to dielectric but also tune the
epsilon-near-zero wavelength (λENZ) over a wide spectral
range. Understanding the role of Al in the transient optical responses
of Ti1–x
Al
x
N under femtosecond excitation is crucial for optoelectronic, photovoltaic,
and photothermal applications. Recently, the electron–phonon
(e–ph) coupling rate and time of TiN have been a controversial
issue, and moreover, little is known about the transient optical properties
of Ti1–x
Al
x
N. In this work, the broadband transient reflectance of highly crystalline
Ti1–x
Al
x
N epitaxial films with various Al concentrations (0 ≤ x ≤ 0.67) is investigated by an ultrafast pump–probe
experiment. With increasing Al concentration, the optical absorption
in the visible to near-infrared region is drastically increased in
the Ti1–x
Al
x
N films, showing great potential to serve as an efficient
absorbing layer for photovoltaic cells. From the carrier dynamics
studies, we found that TiN undergoes wavelength-dependent e–ph
coupling processes with distinctly different lifetimes: sub-picosecond
(≤0.2 ps) in a narrow spectral region near λENZ and a few tens of picoseconds in the metallic region, followed by
a very long heat dissipation process on the nanosecond timescale.
As for Ti1–x
Al
x
N, the spectral region where the ultrafast e–ph coupling
occurs is extended to the whole visible range. While ultrafast and
strong e–ph coupling is advantageous in hot carrier engineering
applications, prolonged preservation of heat in the lattice for a
nanosecond makes TiN and TiAlN emerging photothermal materials with
high conversion efficiency.